دورية أكاديمية
أعرض في EDS

A Biochemical Nickel(I) State Supports Nucleophilic Alkyl Addition: A Roadmap for Methyl Reactivity in Acetyl Coenzyme A Synthase.

التفاصيل البيبلوغرافية
العنوان: A Biochemical Nickel(I) State Supports Nucleophilic Alkyl Addition: A Roadmap for Methyl Reactivity in Acetyl Coenzyme A Synthase.
المؤلفون: Manesis AC; Department of Chemistry and Biochemistry , The Ohio State University , 100 W. 18th Avenue , Columbus , Ohio 43210 , United States., Musselman BW; Department of Chemistry , University of Michigan , 930 N. University Avenue , Ann Arbor , Michigan 48109 , United States., Keegan BC; Department of Chemistry , Trinity University , One Trinity Place , San Antonio , Texas 78212 , United States., Shearer J; Department of Chemistry , Trinity University , One Trinity Place , San Antonio , Texas 78212 , United States., Lehnert N; Department of Chemistry , University of Michigan , 930 N. University Avenue , Ann Arbor , Michigan 48109 , United States., Shafaat HS; Department of Chemistry and Biochemistry , The Ohio State University , 100 W. 18th Avenue , Columbus , Ohio 43210 , United States.
المصدر: Inorganic chemistry [Inorg Chem] 2019 Jul 15; Vol. 58 (14), pp. 8969-8982. Date of Electronic Publication: 2019 Feb 21.
نوع المنشور: Journal Article
اللغة: English
بيانات الدورية: Publisher: American Chemical Society Country of Publication: United States NLM ID: 0366543 Publication Model: Print-Electronic Cited Medium: Internet ISSN: 1520-510X (Electronic) Linking ISSN: 00201669 NLM ISO Abbreviation: Inorg Chem
أسماء مطبوعة: Original Publication: [Easton, Pa.] American Chemical Society.
مواضيع طبية MeSH: Acetyl Coenzyme A/*chemistry , Acetyl Coenzyme A/*metabolism , Nickel/*chemistry , Organometallic Compounds/*chemistry, Azurin/genetics ; Azurin/metabolism ; Catalysis ; Chromatography, Gas ; Gene Expression Regulation, Bacterial ; Kinetics ; Magnetic Phenomena ; Mutation ; Organometallic Compounds/metabolism ; Pseudomonas aeruginosa/enzymology ; Spectrum Analysis
مستخلص: Nickel-containing enzymes such as methyl coenzyme M reductase (MCR) and carbon monoxide dehydrogenase/acetyl coenzyme A synthase (CODH/ACS) play a critical role in global energy conversion reactions, with significant contributions to carbon-centered processes. These enzymes are implied to cycle through a series of nickel-based organometallic intermediates during catalysis, though identification of these intermediates remains challenging. In this work, we have developed and characterized a nickel-containing metalloprotein that models the methyl-bound organometallic intermediates proposed in the native enzymes. Using a nickel(I)-substituted azurin mutant, we demonstrate that alkyl binding occurs via nucleophilic addition of methyl iodide as a methyl donor. The paramagnetic Ni III -CH 3 species initially generated can be rapidly reduced to a high-spin Ni II -CH 3 species in the presence of exogenous reducing agent, following a reaction sequence analogous to that proposed for ACS. These two distinct bioorganometallic species have been characterized by optical, EPR, XAS, and MCD spectroscopy, and the overall mechanism describing methyl reactivity with nickel azurin has been quantitatively modeled using global kinetic simulations. A comparison between the nickel azurin protein system and existing ACS model compounds is presented. Ni III -CH 3 Az is only the second example of two-electron addition of methyl iodide to a Ni I center to give an isolable species and the first to be formed in a biologically relevant system. These results highlight the divergent reactivity of nickel across the two intermediates, with implications for likely reaction mechanisms and catalytically relevant states in the native ACS enzyme.
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معلومات مُعتمدة: R15 GM120641 United States GM NIGMS NIH HHS
المشرفين على المادة: 0 (Organometallic Compounds)
12284-43-4 (Azurin)
72-89-9 (Acetyl Coenzyme A)
7OV03QG267 (Nickel)
تواريخ الأحداث: Date Created: 20190222 Date Completed: 20190809 Latest Revision: 20200225
رمز التحديث: 20221213
مُعرف محوري في PubMed: PMC6635881
DOI: 10.1021/acs.inorgchem.8b03546
PMID: 30788970
قاعدة البيانات: MEDLINE
الوصف
تدمد:1520-510X
DOI:10.1021/acs.inorgchem.8b03546